CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xiaowen Zhang,Hong Wen,Qianwen Huang,Yujiao Tan,Zihao Sun,Yilong Hua,Xiaoyan Wu,Mi Li
Developing a materials to realize the selective adsorption and long-term immobilization of uranium is of great significance for the effective remediation of uranium-containing wastewater. Herein, we half-filled Fe 0 into SGB-NH 2 mesoporous channels to prepare a composite of Fe 0 and amino-functionalized silica (Fe 0 @SGB-NH 2 ), and used to the selective removal of uranium in solution under aerobic conditions . It was found that solutions containing 10 mg/L U(VI) could be purified 98.96% by Fe 0 @SGB-NH 2 in the presence or absence of Na + , K + , Mg 2+ , SO 4 2 − , NO 3 − , HCO 3 − and Cl − at pH 5–9. Compared with Fe 0 , its saturation magnetization decreased from 81.24 emu/g to 0.78 emu/g, while the specific surface area increased from 47.895 m 2 /g to 504.404 m 2 /g, successfully preventing the agglomeration and rapid corrosion of Fe 0 without reducing its activity. More interestingly, the consumption of Fe 0 @SGB-NH 2 was only 1/28 of untreated Fe 0 when identical uranium removal efficiency was achieved. Further mechanistic studies indicated that U(VI) was firstly selectively captured by amino groups on the surface of the material and then reduction or adsorption in the pore, the long and narrow mesoporous channels reduce the possibility of uranium re-oxidation, thereby significantly reducing its re-release efficiency from 21.5% to only 1.73%. Encapsulation of Fe 0 within SGB-NH 2 channels was found to facilitate faster removal rate and higher U(VI) reduction ratio, and reduce uranium re-oxidation, thus benefit the long-term immobilization of uranium in contaminated groundwater.
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Materials Today Chemistry
·
2022
·
IF 7.613
X. Shen,Y. Du,Z. Du,X. Tang,P. Li,J. Cheng,R. Yan,J. Cui
Zeolitic imidazolate framework (ZIF) has recently emerged as a promising material for the encapsulation of enzymes because of their high surface area and facile construction conditions. However, the enzymes are partial even completely inactive after encapsulation owing to the confinement effect and competing coordination, and otherwise, the alkaline environment caused by the protonation effect of 2-methylimidazole also damages enzyme molecules. Herein, a novel glutathione (GSH)-boosted one pot embedding strategy that enabled to rapidly encapsulate enzyme within GSH hybrid MOF (named enzyme@GMOF) with a high embedding efficiency was constructed. Hybrid of GSH and imidazole as synchronous ligands for GMOF to immobilize enzyme can offer sufficient well microenvironment for enzyme exhibiting high activity. The obtained catalysts (CAT@GZIF-67) displayed 9.0-fold higher catalytic activity than traditional ZIF-67 immobilized CAT (CAT@ZIF-67) and superior reusability and storage stability compared with CAT@ZIF-67 and free CAT. As one kind of biomacromolecules, bio-affinity of GSH can create an affinitive microenvironment for enzymes and reduce the influence of other factors during the use of biomacromolecules on their conformation and activity.
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CHEMOSPHERE
·
2023
·
IF 8.8
Xiaoming Zhang,Qi Li,Kai Nie,Kaiting Cao,Qi Liao,Mengying Si,Zhihui Yang,Weichun Yang
Effective remediation of Cr(VI)-contaminated soil with strong alkalinity and high Cr(VI) concentration is a severe challenge. Herein, a proton-buffering montmorillonite-supported sulfidated nano zerovalent iron (nFeS/Fe 0 @H–Mt) was developed for remediation of alkaline Cr(VI)-contaminated soil. The reductive efficiencies of water-soluble Cr(VI) reached 99.7%, 99.3% and 99.8% in three tested soils with initial concentrations of 439.6, 3307.5 and 4626.7 mg kg −1 , respectively, after 15 d of nFeS/Fe 0 @H–Mt treatment. Further speciation analyses demonstrated most available Cr species (exchangeable and carbonate-bound Cr) were transformed into more stable Cr species. The leachable Cr(VI) and total Cr obtained by toxicity leaching procedures decreased to extremely low levels and maintained long-term stability for 120 d. Such superior reductive immobilization performance of FeS/Fe 0 @H–Mt was attributed to the synergistic effect of sulfidated nano zerovalent iron and proton-buffering montmorillonite , which induced the coordination of proton donation and electron transfer . The proton-buffering montmorillonite (H–Mt) could prevent the aggregation of nanoparticles and provide protons to accelerate the corrosion of Fe 0 . In addition, the FeS component improved electron selectivity and facilitated electron transfer of Fe 0 to Cr(VI). Our study demonstrated that the coordination of proton donation and electron transfer significantly enhanced the Cr(VI) reduction under the alkaline condition thus leading to effective remediation of alkaline Cr(VI)-contaminated soil.
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PHILOSOPHICAL MAGAZINE
·
2022
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IF 1.948
Ailian Zhu,Yupeng Xie,Keyou Shi,Min Chen,Jiawei Li,Yimin Zhou,Gaiyuan Chen,Yong Liu
Coal fly ash (hereinafter CFA) was employed to rapidly immobilise Nd-contaminated soil with the addition of TiO2 via microwave sintering technology. The effect of TiO2 doping on the phase composition, microstructure, elemental distribution, density, and chemical durability of the solidified samples was systemically investigated. The results indicated that the Nd element can be incorporated in the matrix with oxyapatite and pyrochlore as TiO2 content increased at 1200°C. Moreover, the sintered sample with the high bulk density and low open porosity was fabricated at a TiO2-doping amount of 7 wt.%. Meanwhile, the as-prepared samples doping with TiO2 exhibited excellent chemical durability. Especially, the sintered sample doping with 3 wt.% TiO2 had the lowest leaching rate (7.97×10−6 g·m−2·d−1 at 28 d). Our investigation reflects that CFA is suitable for Nd-contaminated soil immobilisation via microwave sintering technology and the introduction of TiO2 is conducive to the improvement of densification and chemical durability.
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Frontiers in Microbiology
·
2022
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IF 6.064
Mengkai Hu,Fei Liu,Zhi Wang,Minglong Shao,Meijuan Xu,Taowei Yang,Rongzhen Zhang,Xian Zhang,Zhiming Rao
Sucrose isomerase (SI), catalyzing sucrose to isomaltulose, has been widely used in isomaltulose production, but its poor thermostability is still resisted in sustainable batches production. Here, protein engineering and one-step immobilized cell strategy were simultaneously coupled to maintain steady state for long-term operational stabilities. First, rational design of Pantoea dispersa SI (PdSI) for improving its thermostability by predicting and substituting the unstable amino acid residues was investigated using computational analysis. After screening mutagenesis library, two single mutants (PdSIV280L and PdSIS499F) displayed favorable characteristics on thermostability, and further study found that the double mutant PdSIV280L/S499F could stabilize PdSIWT better. Compared with PdSIWT, PdSIV280L/S499F displayed a 3.2°C-higher T m , and showed a ninefold prolonged half-life at 45°C. Subsequently, a one-step simplified immobilization method was developed for encapsulation of PdSIV280L/S499F in food-grade Corynebacterium glutamicum cells to further enhance the recyclability of isomaltulose production. Recombinant cells expressing combinatorial mutant (RCSI2) were successfully immobilized in 2.5% sodium alginate without prior permeabilization. The immobilized RCSI2 showed that the maximum yield of isomaltulose by batch conversion reached to 453.0 g/L isomaltulose with a productivity of 41.2 g/l/h from 500.0 g/L sucrose solution, and the conversion rate remained 83.2% after 26 repeated batches.
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Advanced Science
·
2022
·Vol. 9
·期 11
·2105556
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IF 17.521
Bin Li,Feng-Fan Lu,Xiao-Wen Gu,Kai Shao,Enyu Wu,Guodong Qian
Developing efficient and stable water adsorbents for adsorption-driven heat transfer technology still remains a challenge due to the lack of efficient strategies to enhance low-pressure water uptakes. The authors herein demonstrate that the immobilization of Lewis basic nitrogen sites into metal–organic frameworks (MOFs) can improve water uptake and target benchmark coefficient of performances (COPs) for cooling and heating. They present the water sorption properties of a chemically stable MOF (termed as Zr-adip), designed by incorporating hydrophilic nitrogen sites into the adsorbent MIP-200. Zr-adip exhibits S-shaped sorption isotherms with an extremely high water uptake of 0.43 g g −1 at 303 K and P / P 0 = 0.25, higher than MIP-200 (0.39 g g −1 ), KMF-1 (0.39 g g −1 ) and MOF-303 (0.38 g g −1 ). Theoretical calculations reveal that the incorporated N sites can serve as secondary adsorption sites to moderately interact with water, providing more binding sites to strengthen the water binding affinity. Zr-adip achieves exceptionally high COPs of 0.79 (cooling) and 1.75 (heating) with a low driving temperature of 70 °C, outperforming MIP-200 (0.78 and 1.53) and KMF-1 (0.75 and 1.74). Combined with its ultrahigh stability, excellent cycling performance, and easy regeneration, Zr-adip represents one of the best water adsorbents for adsorption-driven cooling and heating.
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ACS Applied Nano Materials
·
2023
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IF 5.9
Zhenmao Chen,Yijing Ai,Weiqiang Yang,Li Niu,Qingxiang Wang,Feng Gao
The unique discriminating ability of hydroxyapatite (HAP) to single- and double-stranded nucleic acid implies its potential as a biosensing material for nucleic acid analysis. Herein, a novel immobilization- and label-free electrochemical strategy has been developed for miRNA let-7a detection based on the specific adsorption of magnetic Fe3O4@hydroxyapatite (Fe3O4@HAP) to a duplex structure. Typically, the highly efficient homogeneous reaction between probe DNA (pDNA) and target miRNA let-7a produces the nucleic acid duplex, which is specifically adsorbed on the surface of Fe3O4@HAP. Thereafter, the electroactive intercalator Nile blue (NB) is introduced as the label-free signal molecule and inserts between the stacked base pairs of the pDNA–miRNA duplex. Thus, the Fe3O4@HAP bearing pDNA–miRNA and numerous intercalated NBs are adsorbed by the magnetic glassy carbon electrode, giving rise to an intense sensing signal without the need of nuclease-assisted cyclic amplification. With this advantage, the sensing system shows a wide linear range from 1.0 fM to 100 nM and a low detection limit of 0.051 fM for miRNA let-7a analysis. What is more, the synergy of the base-pairing-driven hybridization, the specific intercalation of NB to the duplex structure, and the selective adsorption of Fe3O4@HAP contribute to a high sensing specificity of the biosensing strategy. The sensing method provides a state-of-the-art strategy for the sensitive and facile bioanalysis and clinical diagnosis of miRNA.
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BIORESOURCE TECHNOLOGY
·
2021
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IF 9.642
Cheng Wang,Xi Chen,Yingying Jiang,Na Li,Ping Zhu,Hong Xu
Facile and green fabrication of reduced graphene oxide on loofah sponge (rGOLS) carrier was applied for cell immobilization of ε-Poly- l -lysine (ε-PL) production. Due to surface properties including large specific surface area, high polarity, and low interaction energy, rGOLS-1 was employed as the optimum rGOLS to enhance immobilization of Streptomyces albulus . Compared with raw LS, batch experiments showed rGOLS-1 facilitated superior cell vitality for ε-PL production due to the presence of reduced graphene oxide. In the sequential fed-batch cultivation of Streptomyces albulus using rGOLS-1 with an aerobic plant fibrous-bed bioreactor (rGOLS-1-AFPB), the maximum ε-PL concentration and productivity reached to 39.2 ± 0.63 g/L and 0.48 g/L/h. The cells immobilized in rGOLS-1 with high vitality and ε-PL production efficiency were reused six times over a period of 624 h. This research afforded an effective approach to enhance the fermentation performance of immobilized cells with the design of an advanced immobilization carrier.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Yuxiao Feng,Yingjie Du,Geling Kuang,Le Zhong,Hongtong Hu,Shiru Jia,Jiandong Cui
Metal–organic frameworks (MOFs), with large specific surface area and tunable porosity, have gained lots of attention for immobilizing enzymes. However, the intrinsic open channels of most reported MOFs are generally smaller than 2 nm, which significantly prevents the passage of enzymes, and the diffusion efficiency of substrates and products. Here we report a new hierarchical micro-mesoporous zeolitic imidazolate framework-8 (ZIF-8) with core–shell superstructure (HZIF-8) using colloidal hydrated zinc sulfate (ZnSO 4 ·7H 2 O) as a soft template for enzyme immobilization. The ZnSO 4 ·7H 2 O forms an aggregation of colloids due to the self-conglobation effect in methanol, which affords a soft template for the formation of HZIF-8. Cytochrome C (Cyt C) was immobilized in interior of HZIF-8 through entrapment during the formation of HZIF-8. The resultant immobilized Cyt C (Cyt [email protected] ) exhibited 4-fold and 3-fold higher activity than free Cyt C and Cyt C encapsulated in conventional microporous ZIF-8 (Cyt [email protected] ), respectively. Meanwhile, the Km value of Cyt [email protected] significantly decreased due to the presence of mesopores compared with Cyt [email protected] , indicating enhanced substrate affinity. After 7 cycles, Cyt [email protected] still maintained 70% of its initial activity whereas Cyt [email protected] only retained 10% of its initial activity. Moreover, the obtained HZIF-8 showed outstanding performance in co-immobilization of multi-enzyme for the detection of glucose.
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Materials Today Communications
·
2023
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IF 3.8
Ruoning Chu,Xiaojie Guo,Yongjun Zhang,Xiaoyu Zhao,Xiantao Xiong,Xiujuan Zhang,Fengyi Zhang,Kun Zhang,Yaxin Wang
Water containing heavy metal ions can be extremely harmful to the environment and human body, thus the development of low-cost and high-efficient adsorbents has an exciting prospect. In this study, lignin/graphene aerogels modified with polydopamine and polyethyleneimine , respectively, were successfully prepared to remove Cr(VI) from aqueous waste. The physicochemical properties of graphene aerogels (GA), lignin/graphene aerogels (LGA), polydopamine-modified lignin/graphene aerogels (LGA@PDA), polyethyleneimine-modified lignin/graphene aerogels (LGA@PEI) were investigated using FT-IR, Raman spectroscopy , XRD , XPS , SEM-EDS, and BET analysis. The results demonstrate that adsorbents have a high specific surface area, an interconnected porous structure, and a large number of oxygen-containing groups, making them particularly favorable for heavy metal adsorption. The effects of GO/lignin ratio, surface modifiers, solution pH, contact time, initial concentration and temperature on the Cr(VI) removal were investigated and compared via batch experiments. Compared with GA (138.74 ± 3.93 mg/g), the adsorption capacity of LGA with GO/LA ratio 40:1 increased to 167.66 ± 4.75 mg/g. Furthermore, the maximum adsorption capacity of LGA@PEI and LGA@PDA rose up to 209.85 ± 3.25 mg/g and 240.39 ± 3.26 mg/mg, respectively. By simulating the experimental data with different kinetic models and isotherm models, the adsorption processes of different lignin-derived aerogels were further explored under various conditions. All types of aerogels fit well with the pseudo-second-order model and Langmuir model. In addition, the XPS results confirm that the chemical reduction of Cr(VI) to Cr(III) also plays a role in the removal of Cr(VI). The results demonstrated that the removal effect of lignin-derived aerogels on Cr(VI) was greatly improved through the multi-functionalized surface modification of LGA with PDA and PEI. Furthermore, the removal efficiency of LGA@PDA and LGA@PEI for Cr(VI) remained stable after repeated regeneration. Therefore, the results of this study indicate that LGA@PDA and LGA@PEI are promising Cr(VI) adsorbents for practical applications in wastewater treatment.
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WASTE MANAGEMENT
·
2023
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IF 8.1
Danni Li,Rui Shan,Jing Gu,Yuyuan Zhang,Xianhai Zeng,Lu Lin,Haoran Yuan,Yong Chen
To relieve the secondary contamination of heavy metals (HMs), the synergistic effect of co-pyrolysis of textile dyeing sludge (DS)/litchi shell (LS) and CaO on the migration of HMs was demonstrated in this study. The proportions of Cu, Zn, Cr, Mn, and Ni in the F4 fraction increased to 75%, 55%, 100%, 50%, and 62% at the suitable CaO dosages. When 10% CaO was added, the RI value of DLC-10% was reduced to 7.89, indicating low environmental risk. The characterizations of the physicochemical properties of biochar provided support for the HMs immobilization mechanism. HMs combined with inorganic minerals or functional groups to form new stable HMs crystalline minerals and complexes to achieve immobilization of HMs. The pH value and pore structure also play an important role in improving the immobilization performance of HMs. In conclusion, the results provided a new direction for the subsequent harmless treatment of HMs-enriched waste.
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Journal of Cleaner Production
·
2021
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IF 9.297
Kai-Qiang He,Chun-Gang Yuan,Yang-Hong Jiang,Yan Li,Xue-Lei Duan,Qi Guo
Some sorbents have been developed for arsenic (As) compounds capture from flue gas . However, most of the conventional sorbents have cost constraints and can cause secondary pollution due to the leaching of arsenic after use. To solve this problem, a new and highly efficient adsorbent for gaseous arsenic was successfully developed in this paper with excellent immobilization performance and low-cost. A series of Mn-supported attapulgite (ATP) composites were fabricated, characterized, and investigated for arsenic capture. The modification of ATP with Mn not only considerably enhanced the adsorption efficiency but also stabilized the adsorbed As in the spent sorbents. SO 2 in flue gas promoted the adsorption performance through As-sulfate binding, whereas NO was beneficial for the oxidation of As(III) to As(V) on the surface of Mn-modified ATP. The incorporation of Mn with ATP generated abundant hydroxylate (OH − ) from hydration and accelerated the formation of As-sulfate compounds, which was beneficial for physical encapsulation. The results of the toxicity characteristic leaching procedure and sequential extraction test revealed that adsorbed As could be considerably immobilized by the sorbent with low leaching ability. Mn modification changed more As into inert fractions and consequently inhibited release from spent sorbents, which considerably reduced the risks of secondary pollution. The developed composite can be potentially used as a new efficient sorbent for gaseous arsenic capture in flue gas.
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